Topology induced crossover between Langevin, subdiffusion, and Brownian diffusion regimes in supercooled water

Zhu, Kaicheng; Naserifar, Saber; Goddard, III, William A.; Su, Haibin

doi:10.1039/d2cp04645h

Topology induced crossover between Langevin, subdiffusion, and Brownian diffusion regimes in supercooled water

Journal Article · Mon Mar 20 00:00:00 EDT 2023 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/d2cp04645h· OSTI ID:2421864

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Hong Kong University of Science and Technology (HKUST) (Hong Kong); OSTI
California Institute of Technology (CalTech), Pasadena, CA (United States)
Hong Kong University of Science and Technology (HKUST) (Hong Kong)

Despite extensive studies of supercooled water, it remains challenging to understand its peculiar dynamic anomalous properties. In this work, we integrated full atomistic simulations of supercooled water over the temperature range of room temperature to 200 K using a quantum-mechanics-based polarizable force field with the dressed dynamics method that couples fast collision events and slow reorganization dynamics of hydrogen-bond networks. Our analysis unveils the salient multiscale features in the transient relaxation dynamics of supercooled water. A classical Langevin behavior dominates at fast timescales, while long-time relaxations unveil two different activation barriers in two temperature regions: below and above 230 K. The modulation of the entropy spectrum by temperature is elucidated in terms of a three-state model underlined by the complexity of the water dynamics associated with a topological transition of a strong hydrogen-bond network. This state-dependent network topology is quantitatively characterized by power-law exponents of inverse network connectivity from 200 to 298 K. Finally, this work provides valuable guidance for further studies on the transient relaxation dynamics of supercooled water.

View Accepted Manuscript (DOE)

Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0021266

OSTI ID:: 2421864

Alternate ID(s):: OSTI ID: 1967509

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 15 Vol. 25; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Topology induced crossover between Langevin, subdiffusion, and Brownian diffusion regimes in supercooled water

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